Chinese J. Chem. Eng.

, 14(3) 364-370 (2006)

Correlation of Viscosities for Alkane, Aromatic and Alcohol Family at

High Pressure by Modified Tait Equation*

w
XUAN Aiguo( % f !Sl)ab***, WU Yuanxin( Z %)', PENG Changjun( @ )", MA Pei-
WANG Cunwen(Z..kft)b and ZHANG Liangjun( $#hh$)d
sheng(4 8jk)",
a School of Chemical Engineering and Technology ,Tianjin University ,Tianjin300072,China
Department of Chemical Engineering, Wuhan Institute of Chemical and Technology, Wuhan 430073,China
Department of Chemistry, East China University of Science and Technology, Shanghai 200237, China
Hubei Key Laboratory of Novel Chemical Reactor and Green Chemical Technology, Wuhan 430073,China

Abstract A new model was proposed to calculate the viscosity of fluids under the pressure ranging from 0.1 to
llOMPa by improving the Tait equation, in which the viscosity p of liquids was linked with activation volume P.
The model with two adjustable parameters a and B was applied in calculating viscosities for alkane, aromatic and
alcohol family at high pressure. Results show that calculated values of viscosity are in good agreement with the ex-
perimental ones, and the average relative deviations for alkanes, aromatics and alcohols are 0.56%. 0.31% and
0.66%, respectively. Besides, the errors correlated by the model proposed in this paper were equivalent to the ones
from the pure empirical Tait equation, and obviously superior to those from Eyring equation.
Keywords viscosity, model, high pressure, Tait equation, activation volume

1 INTRODUCTION studies of Kashiwagi and Makita'", Tanaka et ~ 1 . " ~ ~

It is of fundamental importance to obtain accu-
rate viscosity data of liquids over wide ranges of tem-
perature and pressure for the development and opti-
mization of industrial processes. On the other hand,
the viscosity of pure components is adopted as an in-
put parameter in establishing the most reliable viscos-
ity models of liquid mixtures. Therefore, there is an
increasing demand of accurate models for pure liquid
viscosities, particularly under high-pressure condi-
tion~"-~].
It is convenient to calculate the viscosity of
high-pressure pure liquid by considering the viscosity
value as the molar volume in the P-V-T relationship of
a conventional equation of state. Several models about
the pressure dependence on pure fluid and their mix-
ture viscosity by applying the Pate1 and TejaL6]and
Peng and Robinson[71equations of state were proposed
by Guo et ~ 1 . ' ~ It' . must be pointed out that all these
models are pure-empirical. Tait equation was one of
the typical examples, which can be not only satisfied
with the correlation of high-pressure liquid volume,
but also is suitable to correlate high pressure liquid
viscosity. The form of Tait equation was taken on the
and Assael et al.'"]. Theoretically, the pressure is con-
sidered to depend on viscosity strickly, as proposed by
Glasstone et al."*].The volume of activation can be
related to pressure and viscosity in their work. How-
ever, under the actual conditions, the liquid volume of
activation is treated as a parameter independent of
pressure, because it is hard to be cal~ulated"~-'~~.
Progress have been made in the study of viscos-
ity of liquids and liquid mixtures, but there is no
widely accepted simple theoretical method for liquid
viscosity. The development of model based on differ-
ent background and framework, theoretical and em-
pirical, is accepted at the present stage. The aim of this
work is to present a new attempt for viscosity calcula-
tion of pure liquids, from atmospheric up to high
pressures. The model with two adjustable parameters
is started in terms of Eyring viscosity equation. The
key was to adopt a modified Tait equation to estimate
the activation volume in the Eyring viscosity equation.
2 DESCRIPTION OF THE MODEL
Pressure dependence of viscosity is often de-
scribed in terms of the volume of activation as

Received 2005-08-29, accepted 2006-01-19.

* Supported by the National Natural Science Foundation of China (No.20476083) and the Natural Science Foundation of Hubei
Province (No.2002AB065).
** To whom correspondence should be addressed. E-mail: jixiang_er@163.com
 Correlationof Viscosities for Alkane, Aromatic and Alcohol Family at High Pressure by Modified Tait Equation
p = Aexp( g)
where p, A, f ,R, T and P are the dynamic viscosity
of Newtonian liquids, a pre-factor, the volume of ac-
tivation, the gas constant, temperature and pressure,
respectively. If it is supposed that the pre-factor A is
dependent on temperature only, the viscosity of the
reference pressure at the same temperature can be then
calculated:
: : pL I
pEf= Aexp -
where the subscript ref is refered to the reference state.
Generally, the value of PEfis O.1MPa or 0.1OlMPa.
From Eqs.(l) and (2), the following equation can be
obtained:
For a given fluid at constant temperature,
PEfVZf / RT= a , a constant. Therefore,
Up to the present, no reliable method is adopted
to calculate the value of the volume of activation.
Here, Tait equation can be adopted to estimate the
volume of activation.
It is well known that the Tait equation can repro-
duce PVT relation of many polymer melts"51. The
specific volume v for polymer melt at high pressure
can be usually calculated by the following Tait equa-
tion[161.
v(PJ) =1-0.0894ln[l+P/B(t)] (5)
v(0,t)
Obviously, the pressure of reference state in the
Tait equation is zero. However, the phase state
changes for the liquid with small molecules when the
reference pressure is zero. Hence, Eq.(5) must be
modified to meet the requirement of its application. In
this study, one parameter K replaces the constant
0.0894 and another parameter p substitutes B(t).
Therefore,
Putting Eq.(6) into Eq.(4), we obtain
365
(7)
Equation (7) can be used to calculate the viscos-
ity of fluid at high pressure, in which the reference
state is the atmospheric pressure, because the viscosity
at O.1MPa is usually known. Three parameters must
be regressed. However, it is discovered from experi-
ments that K is about 0.5 at different temperatures.
Thus, for simplicity, K is regarded as a constant. The
final expression of the model is
(8)
Eq.(8) is a new model, where both parameters a and /?,
which are function of temperature and independent of
pressure, are regressed by the experimental data of
viscosity.
3 RESULTS A N D DISCUSSION
The model parameters and the correlated results
by using Eq.(8) are listed in Table 1. For comparison,
the results correlated by Kashiwagi and Makita"], Ta-
n k a et ~ 1 . "and
~ ~Assael et uf.'"] with the modified
Tait equation (or Tait equation) and those correlated
by Eyring viscosity equation under the consideration
of pressure (or Eyring equation) are also given in Ta-
ble 1[17-271
Pressure dependence of viscosity of different or-
ganic substances at 298.15K is illustrated in Fig.1.
And the experimental data for n-hexane and n-heptane
were re-produced by the model parameters of Kashi-
wagi and Makita. The agreement between experimental
and calculated viscosity was rather satisfactory. The
deviations obtained in this work for n-hexane,
n-heptane, n-octane(297.95K), n-decane(297.95K),
n-dodecane and n-hexdecane were 0.13%, 0.09%,
0.82%, 0.80%,0.10% and 0.25%, respectively. The
results correlated by Tait equation were 0.2%, 0.3%,
0.83%, 0.81%, 0.30% and 0.25%, respectively. And
the results by Eyring equation were 1.64%, 1.42%,
1.32%, 1.66%, 1.47% and 1.87%, respectively. It in-
dicates that our model is comparable to Tait equation,
and superior to Eyring equation.
A comparison of viscosity between the experi-
mental data and the calculated results with our model
for n-decane and rn-xylene at different temperatures is
Chinese J. Ch. E. 14(3)364 (2006)
366 Chinese J. Ch. E. 0'01.14, No3)

n b l e 1 The model parameters and correlated results

Dev', 8
Substance T, K P,m a a x lo4 j~,ma References
E44.(8) Tait equation Eyring equation
283.15 0.1-69 6.592 75.979 0.44 0.37 0.7 1
298.15 0.1-73 7.310 64.363 0.80 1.48 0.24
methanol [8,171
323.15 0.1-69 4.295 487.548 0.49 0.15 0.55
348.15 0.1-69 4.439 143.284 1.02 1.37 0.76
298.15 0.1-79 6.642 204.928 0.12 0.53 0.43
ethanol [8,17,181
323.15 0.1-59 9.818 55.113 0.75 0.61 0.60
283.15 0.1-118 8.628 171.987 0.16 0.17 1.42
1-propano1 298.15 0.1-118 7.913 214.963 0.25 0.39 1.42 [3,10,17,18]
323.15 0.1-118 8.660 169.521 0.04 0.07 1.41
298.15 0.1-118 10.262 173.228 1.03 0.22 1.95
2-propanol [101
323.15 0.1-118 10.302 165.948 0.18 0.09 1.63
323.15 0.1-69 17.708 246.245 0.24 0.24 1.65
2-methyl-2-pmpanol
348.15 0.1-30 21.821 54.537 0.42 0.44 1.87
n-butan01 298.15 0.1-53 13.854 37.656 3.39 3.42 5.68 [3,171
298.15 0.1-110 8.623 363.672 0.51 0.52 0.72
303.15 0.1-110 8.633 322.880 0.02 0.2 0.78
benzene [3.9,191
323.15 0.1-169 9.674 192.561 1.81 1.84 1.54
348.15 0.1-178 8.683 285.178 1.63 1.53 2.05
248.32 0.1-81 8.253 710.921 0.20 0.21 0.89
273.3 0.1-81 8.045 334.839 0.11 0.11 0.76
298.15 0.1-203 7.434 531.147 0.73 0.83 1.09
toluene 303.15 0.1-252 7.751 305.572 0.24 0.27 0.53 [9,11,19,20]
323.15 0.1-252 7.607 321.054 0.42 0.32 0.65
348.15 0.1-252 7.138 382.054 1.89 1.92 2.05
373.15 0.1-78 7.882 623.395 0.76 0.76 0.87
298.15 0.1-110 7.559 350.129 0.02 0.2@ 0.64
303.15 0.1-110 7.671 306.168 0.02 0.3@ 0.73
ethylbenzene
323.15 0.1-110 7.579 260.806 0.04 0.2@ 0.82
191
348.15 0.1-110 7.997 191.744 0.06 0.3@ 1.06
298.15 0.1-47 7.733 1411.322 0.22 0.22 0.24
mesitylene
313.15 0.1-47 8.033 338.539 0.06 0.06 0.18
298.15 0.1-110 7.534 414.436 0.01 0.2@ 0.57
303.15 0.1-110 7.598 351.285 0.02 0.3@ 0.65
m-xylene [91
323.15 0.1-110 7.427 304.825 0.02 0.2@ 0.7 1
348.15 0.1-110 7.819 206.128 0.05 0.3@ 0.98
298.15 0.1-110 8.634 344.315 0.02 0.3@ 0.75
303.15 0.1-110 8.424 ' 370.834 0.02 0.3@ 0.69
o-xylene [91
323.15 0.1-110 8.267 312.859 0.02 0.3@ 0.78
348.15 0.1-110 8.265 232.751 0.04 0.3@ 0.95
298.15 0.1-110 8.637 160.819 0.09 0.2@ 1.26
303.15 0.1-110 8.412 227.310 0.04 0.3@ 0.98
p-xylene [91
323.15 0.1-110 8.158 251.681 0.03 0.2@ 0.89
348.15 0.1-110 8.067 237.516 0.04 0.3@ 0.93
n-pentane 297.95 0.1-25 1.023 114.853 0.85 0.53 0.98 [11,211

June, 2006
 Correlation of Viscosities for Alkane, Aromatic and Alcohol Family at High Pressure by ModiFied W t Equation 367

Tgble 1 (continued)
Dev', %
Substance T, K P,Wa a~104 B,Wa References
Fq(8) Tait equation Eyring equation
298.15 0.1-110 10.377 139.925 0.13 0.2@ 1.64
303.15 0.1-110 10.339 138.675 0.14 0.2@ 1.63
n-hexane
323.15 0.1-110 11.350 117.017 0.20 0.4@ 1.97
333.15 0.1-110 12.174 100.133 0.29 0.4@ 2.25
298.15 0.1-110 13.059 377.844 0.03 0.2@ 1.06
303.15 0.1-110 13.105 266.349 0.05 0.2Q 1.38
cyclohexane 323.15 0.1-1 10 12.602 252.442 0.05 0.3@ 1.38 [3,9,221
348.15 0.1-110 12.822 203.638 0.08 0.5@ 1.62
373.15 0.1-200 13.253 173.361 0.08 0.08 O.%
298.15 0.1-110 10.149 172.392 0.09 0.3' 1.42
303.15 0.1-110 10.459 155.459 0.11 0.3Q 1.56
n-heptane
323.15 0.1-110 11.037 131.435 0.16 0.3@ 1.79
348.15 0.1-110 12.194 107.717 0.26 0.4@ 2.18
297.95 0.1-25 13.571 133.5543 0.82 0.83 1.32
313.05 0.1-25 14.442 40.1793 0.32 0.52 1.09
328.05 0.1-25 12.112 14972.443 1.61 5.22 2.87
n-octane [241
343.15 0.1-25 12.301 297.445 1.53 4.59 4.99
358.25 0.1-25 18.453 21.929 1.75 1.72 1.98
373.35 0.1-25 15.882 35.559 0.88 0.89 1.03
303.15 0.1-65 10.536 268.431 0.10 0.10 1.32
n-nonane
323.15 0.1-69 10.892 172.147 0.08 0.09 1.42
297.95 0.1-25 12.062 63.747 0.80 0.81 1.66
313.05 0.1-25 16.011 23.981 0.51 0.59 1.55
328.05 0.1-25 16.014 26.556 0.37 0.42 1.34
n-decane
343.15 0.1-25 16.465 25.723 0.78 0.77 1.65
358.25 0.1-25 17.123 29.2965 0.36 0.39 1.32
373.35 0.1-25 79.860 84776.407 1.19 1.19 2.54
298.15 0.1-30 13.254 305.131 0.25 0.25 1.87
n-hexadecane 323.15 0.1-148 12.543 280.052 0.48 0.38 1.46 ~ 7 1
348.15 0.1-150 12.093 247.615 0.79 0.65 1.65
298.15 0.1-92 12.614 235.837 0.10 0.3 1.47
323.15 0.1-150 11.651 251.732 0.32 0.35 1.69
348.1 0.1-422 9.998 407.379 2.01 2.21 1.35
n-dodecane 298.27 0.1-1 19 12.094 283.492 0.1 1 0.08 1.46 [7,15,271
323.35 0.1-261 10.891 354.752 1.01 1.01 1.98
373.21 0.1-501 9.492 422.211 2.77 2.78 1.57
348.15 0.1-150 11.380 225.492 0.39 0.37 1.55
total average 0.72 0.87 1.46
error 0.43@ 0.68@ 1.36@

@ Given by Ref.[7].
@ Error values were calculated by all the data from related references, including the error from Kashiwagi's model.

Chinese J. Ch. E. 14(3) 364 (2006)

368 Chinese J. Ch. E. (Vol. 14, No.3)

5.00 I

1.2 -

1.0 -
3.01 v1
b
E
i2.01 0.6
0.4 -
1.oo

I I I I I I I
0.2 1
0 20 40 60 80 100 120 0 30 60 90 120
P , MPa P, MPa
Figure 1 Pressure dependence of viscosity of alkanes at
Figure 3 Pressure dependence of viscosity of m-xylene at
298.15K
Merent temperature
,and the
(Symbols mean the literature datat3.7.Q~15.'e.23~2426.271 (Symbols are the literature dadQ1and the lines are the correla-
lines are the correlation results with present mode)
tion results with preasent mode)
0 n-hexane; A n-heptane; 0 n-octane(297.95K);
+298.15K; 0 303.153, A 323.153, 0 348.15K
+
A n-decane(297.95K); n-dodecane; W n-hexdecane

shown in Figs.2 and 3. A good agreement is ob-

served between the experimental values and those
calculated from Fig.2 and Table 1.

1.20 I I

1.oo

v1 0.80

0.60 0 20 40 60 80 100 120 140

d P, MPa
0.40
Figure 4 Pressure dependence of viscosity of alcohols at

o.20 t 298.15K
(Symbols mean the literature data[3'8*'0"7"81
, and the lines are
0 5 10 15 20 25 30 the correlation results with present model)
P, MPa 0 methanol; A ethanol; 0 I-propanol; A 2-propanol
Figure 2 Pressure dependence of viscosity of n-decane at
different temperature
rectly reported in their paper. The error from our
(Symbols are the literature dadz6]and the lines are the correla-
tion results with present model) model was about 0.72% if the error from Kashiwagi's
0 297.95K; A 313.053, +
328.05K; model was subtracted, while the error from Tait equa-
0 343.15K3: A 358.25K tion and Eyring equation were 0.87% and 1.46%, re-
spectively. If all the data were taken into consideration,
As illustrated in Fig.4, the experimental and cal- the total mean error correlated from our model was
culated values of the viscosities for n-alcohols at 0.43%, yet those from Tait equation and Eyring equa-
298.15K are presented. Pressures are in the range from tion were 0.68% and l .36%, respectively. On the other
O.1MPa to 120MPa for 1-propanol and 2-propanol, to hand, Kashiwagi and Makita have found that the de-
80MPa for methanol, and to 60MPa for ethanol. It is rivative of Tait equation with respect to pressure is
found that our model can reproduce commendably always negative"], which means that the Tait equation
P-p-T relations of alcohol family. is inapplicable to liquids whose viscosity increases
The results correlated using our model for other rapidly with pressure. Our model is better than Tait
liquids are also listed in Table1. A portion of data were equation, and is obviously superior to Eyring equation.
calculated from the model suggested by Kashiwagi This is because the activation volume in Eyring equa-
and Makita"] because the experimental data were di- tion is regarded as a parameter independence of the
June, 2006
 Correlation of Viscosities for Alkane, Aromatic and Alcohol F d y at High Pressure by Modified ‘hit Equation
pressure.but it should be a function of temperature and
pressure.
It should be noted that Eq.(8) can be only used to
correlate the viscosity with pressure at fixed tempera-
ture. Hence, when the temperature is changed in the
system, the value pmf,the reference viscosity, must be
known at O.lMPa, or it must be regressed as a pa-
rameter by experimental data.
4 CONCLUSIONS
On the basis of the pressure equation of viscosity
and modified Tait equation, a novel model for the dy-
namic viscosity of pure liquid at high pressures was
developed. Adopting a modified Tait equation to es-
timate the volume of activation is the core of the
model. The resulting expression of the model contains
two adjustable parameters, a and p. The proposed
model is successfully applied to correlate experimen-
tal viscosity data of alkane, alcohol and aromatic fam-
ily at high pressures. The results calculated by our
model are comparable to that from Tait equation, and
superior to that by Eyring equation.
NOMENCLATURE
Dev average relative deviation, %
P pressure, MPa
T temperature, K
activation volume, m3.mo1-’
a, model parameter
P viscosity, r n P a s
Superscripts and Subscripts
cal calculated property
exp experimental property
ref reference state
# activated state
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